The effects of MoOx decoration on the selective hydrogenation of crotonaldehyde over MoOx-promoted Ir/TUD-1 catalysts

The effects of MoOx decoration on the selective hydrogenation of crotonaldehyde over MoOx-promoted Ir/TUD-1 catalysts
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MoOx 修饰对 MoOx 促进的 Ir/TUD-1 催化剂上巴豆醛选择性加氢的影响

DOI:
10.1016/j.jcat.2019.11.007
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发表时间:
2020
影响因子:
7.3
通讯作者:
Lu Ji-Qing
Lu Ji-Qing
中科院分区:
化学1区
文献类型:
--
作者:
Xu Yu-Meng;Zheng Wan-Bin;Hu Yi-Ming;Tang Cen;Jia Ai-Ping;Lu Ji-Qing

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测试了一系列 MoOx 促进的 Ir/TUD-1 催化剂用于巴豆醛的液相选择性加氢。促进后的催化剂比未促进的催化剂表现出更高的活性和选择性,其中在 Ir-0.1Mo/TUD-1 上获得了最佳性能(巴豆醇产率为 86.7%,周转数为 325.7 h−1)。 TUD-1的大孔径有利于反应物的扩散,因此负载型催化剂比商业SiO2负载型催化剂活性更高。表征结果揭示了 MoOx 对 Ir 粒子的修饰,这改变了催化剂的形态和电子特性。这种修饰导致Ir-MoOx界面位点的产生,改变了巴豆醛分子的吸附和活化,从而提高了活性和选择性。然而,当MoOx含量较高时,Ir表面被MoOx完全覆盖,导致巴豆醛的吸附较强,并且用于解离H2的表面Ir原子较少,从而导致活性下降。
A series of MoOx-promoted Ir/TUD-1 catalysts were tested for liquid phase selective hydrogenation of crotonaldehyde. The promoted catalysts showed higher activity and selectivity than the unpromoted one, with the best performance being obtained on an Ir-0.1Mo/TUD-1 (with a crotyl alcohol yield of 86.7% and a turnover number of 325.7 h−1). The large pore sizes of the TUD-1 is beneficial to the diffusion of the reactant and thus the supported catalyst is more active than that supported on the commercial SiO2. The characterization results revealed decoration of Ir particles by MoOx, which altered the morphologies and electronic properties of the catalysts. Such decoration resulted in the generation of Ir-MoOxinterfacial sites, which altered the adsorption and activation of crotonaldehyde molecule and brought up enhanced activity and selectivity. However, at high MoOxcontent, the Ir surface was fully covered by MoOx, which results in strong adsorption of crotonaldehyde and fewer surface Ir atoms for H2dissociation and thus declined activity.
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